“…7 Compared to other benchmark porous materials such as zeolites, amorphous POPs, and MOFs, COFs have unparalleled structural advantages including ultralow density, regular networks, high porosity, exceptional structural modularity, and superb synthetic versatility, which underpin their broad applications in gas storage, catalysis, energy storage, water harvesting, environmental remediation, etc. [8][9][10][11] Since the first report of using COFs as iodine adsorbents in 2017, 12 enormous scientific efforts have been devoted to the fabrication of high-performance COF adsorbents through three main routes: (1) de novo synthesis of COF adsorbents containing iodine affinity sites such as imine, [13][14][15] hydrazone, 16 cationic species, 17 amino, 18 hydrazides, 19 thiophene, 20 tetrathiafulvalene, 21 phosphine; 22 (2) grafting ionic groups onto already-synthesized COFs by post-synthetic modification; 23 and (3) constructing hierarchically porous COFs through supercritical CO 2 drying, 24 freezedrying, 25 and template-assisted modulated synthesis. 26 Despite substantial advances, the synthesis of COF adsorbents still heavily relies on conventional solvothermal synthesis, which entails multiday synthesis, the usage of toxic organic solvents, high temperatures, and anaerobic conditions.…”